Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites

Hydrogen sulfide is removed from natural gas via adsorption on zeolites. The process operates very effectively, but there is still potential for improvement. Therefore, in this article, the adsorption of hydrogen sulfide was investigated on eight LTA zeolites with different cation compositions. Star...

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Main Authors: Annika Starke, Christoph Pasel, Christian Bläker, Tobias Eckardt, Jens Zimmermann, Dieter Bathen
Format: Article
Language:English
Published: Hindawi - SAGE Publishing 2021-01-01
Series:Adsorption Science & Technology
Online Access:http://dx.doi.org/10.1155/2021/5531974
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spelling doaj-d573d6922abd4cf99361b51a53ee66a62021-06-07T02:13:30ZengHindawi - SAGE PublishingAdsorption Science & Technology2048-40382021-01-01202110.1155/2021/5531974Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA ZeolitesAnnika Starke0Christoph Pasel1Christian Bläker2Tobias Eckardt3Jens Zimmermann4Dieter Bathen5University of Duisburg-EssenUniversity of Duisburg-EssenUniversity of Duisburg-EssenBASF Catalysts Germany GmbHChemiewerk Bad Köstritz GmbHUniversity of Duisburg-EssenHydrogen sulfide is removed from natural gas via adsorption on zeolites. The process operates very effectively, but there is still potential for improvement. Therefore, in this article, the adsorption of hydrogen sulfide was investigated on eight LTA zeolites with different cation compositions. Starting with the zeolite NaA (4 A), which contains only Na+ cations, the Ca2+ cation content was gradually increased by ion exchange. Equilibrium isotherms from cumulative breakthrough curve experiments in a fixed-bed adsorber at 25°C and 85°C at 1.3 bar (abs.) were determined in the trace range up to a concentration of 2000 ppmmol. From a comparison of the isotherms of the different materials, a mechanistic proposal for the adsorption is developed, taking into account the specific positions of the cations in the zeolite lattice when the degree of exchange is increased. The shape of the isotherms indicates two energetically different types of adsorption sites. It is assumed that two mechanisms are superimposed: a chemisorptive mechanism with dissociation of hydrogen sulfide and covalent bonding of the proton and the hydrogen sulfide ion to the zeolite lattice and a physisorptive mechanism by electrostatic interaction with the cations in the lattice. As the degree of exchange increases, the proportion of chemisorption sites seems to decrease. Above an exchange degree of 50%, only evidence of physisorption can be found. It is shown that this finding points to the involvement of weakly bound sodium cations at cation position III in the chemisorption of hydrogen sulfide.http://dx.doi.org/10.1155/2021/5531974
collection DOAJ
language English
format Article
sources DOAJ
author Annika Starke
Christoph Pasel
Christian Bläker
Tobias Eckardt
Jens Zimmermann
Dieter Bathen
spellingShingle Annika Starke
Christoph Pasel
Christian Bläker
Tobias Eckardt
Jens Zimmermann
Dieter Bathen
Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
Adsorption Science & Technology
author_facet Annika Starke
Christoph Pasel
Christian Bläker
Tobias Eckardt
Jens Zimmermann
Dieter Bathen
author_sort Annika Starke
title Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
title_short Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
title_full Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
title_fullStr Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
title_full_unstemmed Impact of Na+ and Ca2+ Cations on the Adsorption of H2S on Binder-Free LTA Zeolites
title_sort impact of na+ and ca2+ cations on the adsorption of h2s on binder-free lta zeolites
publisher Hindawi - SAGE Publishing
series Adsorption Science & Technology
issn 2048-4038
publishDate 2021-01-01
description Hydrogen sulfide is removed from natural gas via adsorption on zeolites. The process operates very effectively, but there is still potential for improvement. Therefore, in this article, the adsorption of hydrogen sulfide was investigated on eight LTA zeolites with different cation compositions. Starting with the zeolite NaA (4 A), which contains only Na+ cations, the Ca2+ cation content was gradually increased by ion exchange. Equilibrium isotherms from cumulative breakthrough curve experiments in a fixed-bed adsorber at 25°C and 85°C at 1.3 bar (abs.) were determined in the trace range up to a concentration of 2000 ppmmol. From a comparison of the isotherms of the different materials, a mechanistic proposal for the adsorption is developed, taking into account the specific positions of the cations in the zeolite lattice when the degree of exchange is increased. The shape of the isotherms indicates two energetically different types of adsorption sites. It is assumed that two mechanisms are superimposed: a chemisorptive mechanism with dissociation of hydrogen sulfide and covalent bonding of the proton and the hydrogen sulfide ion to the zeolite lattice and a physisorptive mechanism by electrostatic interaction with the cations in the lattice. As the degree of exchange increases, the proportion of chemisorption sites seems to decrease. Above an exchange degree of 50%, only evidence of physisorption can be found. It is shown that this finding points to the involvement of weakly bound sodium cations at cation position III in the chemisorption of hydrogen sulfide.
url http://dx.doi.org/10.1155/2021/5531974
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